Abstract
Electrochemical reduction of NO not only offers an attractive alternative to the Haber-Bosch process for ambient NH3 production but mitigates the human-caused unbalance of nitrogen cycle. Herein, we report that MoS2 nanosheet on graphite felt (MoS2/GF) acts as an efficient and robust 3D electrocatalyst for NO-to-NH3 conversion. In acidic electrolyte, such MoS2/GF attains a maximal Faradaic efficiency of 76.6 % and a large NH3 yield of up to 99.6 mu mol cm(-2) h(-1). Using MoS2 nanosheet-loaded carbon paper as the cathode, a proof-of-concept device of Zn-NO battery was assembled to deliver a discharge power density of 1.04 mW cm(-2) and an NH3 yield of 411.8 mu g h(-1) mg(cat.)(-1). Calculations reveal that the positively charged Mo-edge sites facilitate NO adsorption/activation via an acceptance-donation mechanism and disfavor the binding of protons and the coupling of N-N bond.